Temperature-Dependent Intensity Modulated Two-Photon Excited Fluorescence Microscopy for High Resolution Mapping of Charge Carrier Dynamics

IF 3.7 Q2 CHEMISTRY, PHYSICAL ACS Physical Chemistry Au Pub Date : 2023-07-07 DOI:10.1021/acsphyschemau.3c00013
Qi Shi, Pushpendra Kumar and Tönu Pullerits*, 
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引用次数: 2

Abstract

We present a temperature-dependent intensity modulated two-photon excited fluorescence microscopy technique that enables high-resolution quantitative mapping of charge carrier dynamics in perovskite microcrystal film. By disentangling the emission into harmonics of the excitation modulation frequency, we analyze the first and second order charge carrier recombination processes, including potential accumulation effects. Our approach allows for a quantitative comparison of different emission channels at a micrometer resolution. To demonstrate the effectiveness of the method, we applied it to a methylammonium lead bromide perovskite microcrystal film. We investigated the temperature-dependent modulated imaging, encompassing the exciton dissociation-association and charge carrier trapping-detrapping equilibrium. Additionally, we explored the potential freezing out of traps and the phase transition occurring at low temperatures.

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用于电荷载流子动力学高分辨率映射的温度相关强度调制双光子激发荧光显微镜。
我们提出了一种依赖温度的强度调制双光子激发荧光显微镜技术,该技术能够对钙钛矿微晶膜中的电荷载流子动力学进行高分辨率定量映射。通过将发射分解为激励调制频率的谐波,我们分析了一阶和二阶电荷载流子复合过程,包括电势累积效应。我们的方法允许在微米分辨率下对不同的发射通道进行定量比较。为了证明该方法的有效性,我们将其应用于甲基铵-溴化铅钙钛矿微晶膜。我们研究了与温度相关的调制成像,包括激子离解缔合和电荷载流子捕获-去俘获平衡。此外,我们还探索了陷阱的潜在冻结和低温下发生的相变。
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CiteScore
3.70
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期刊介绍: ACS Physical Chemistry Au is an open access journal which publishes original fundamental and applied research on all aspects of physical chemistry. The journal publishes new and original experimental computational and theoretical research of interest to physical chemists biophysical chemists chemical physicists physicists material scientists and engineers. An essential criterion for acceptance is that the manuscript provides new physical insight or develops new tools and methods of general interest. Some major topical areas include:Molecules Clusters and Aerosols; Biophysics Biomaterials Liquids and Soft Matter; Energy Materials and Catalysis
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Issue Publication Information Issue Editorial Masthead Roundabout Mechanism of Ion–Molecule Nucleophilic Substitution Reactions Ultrafast Spin Relaxation of Charge Carriers in Strongly Quantum Confined Methylammonium Lead Bromide Perovskite Magic-Sized Clusters Direct Detection of Bound Water in Hydrated Powders of Lysozyme by Differential Scanning Calorimetry
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